Single‐Step Conversion of Metal Impurities in CNTs to Electroactive Metallic Nitride Nanoclusters for Electrochemical CO 2 Reduction

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Abstract
A novel single‐step low‐temperature pyrolysis method is developed to efficiently remove encapsulated Ni nanoparticles (NPs, 10–50 nm) from both regular‐grade (3 N‐NCs, along with some metallic Ni‐NCs. The treated materials demonstrate exceptional electroactivity toward CO 2 reduction to CO, with the best‐performing CNT‐PTFE‐Mel‐650 sample achieving an ultra‐low onset overpotential of −19 mV and 98% CO selectivity in a current density range of 100–700 mA cm −2 . This NC catalyst demonstrates 25% lower voltage at 700 mA cm −2 compared to the single atom catalyst (SAC) control. Experimentally verified ab initio molecular dynamics (AIMD) models are simulated, and subsequent density functional theory (DFT) calculations further support the thermodynamic stability of Ni 3 N‐NCs and their favorability for CO 2 reduction. This work establishes a new method for creating ligand‐free electroactive NCs for efficient electrochemical reactions.
Funding Information
  • National Science Foundation (CBET‐2151049)
  • U.S. Department of Energy
  • Office of Science
  • Basic Energy Sciences (DE‐AC02‐76SF00515)

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